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Catalysis: From Principles to Applications

Matthias Beller (Editor), Albert Renken (Editor), Rutger A. van Santen (Editor)
ISBN: 978-3-527-32349-4
664 pages
September 2012
Catalysis: From Principles to Applications (352732349X) cover image

Catalysis has revolutionized the chemical industry as catalysts are used in the production of most chemicals, resulting in a multi-billion euro business. This advanced textbook is a must-have for all Master and PhD students in the field as it adopts a unique interdisciplinary approach to the topic of catalysis. It presents a collection of chapters that explain the fundamentals of catalysis as the area has developed over the past decades and introduces new catalytic systems that are of becoming of increasing current importance.

It covers all the essential principles, ranging from catalytic processes at the molecular level to catalytic reactor design and includes several case studies illustrating the importance of catalysts in the chemical industry.

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List of Contributors XVII

Preface XXI

Part I Basic Concepts 1

1 Catalysis in Perspective: Historic Review 3
Rutger van Santen

1.1 History of Catalysis Science 3

1.2 The Development of Catalytic Processes: History and Future 11

1.3 Fundamental Catalysis in Practice 13

1.4 Catalyst Selection 13

1.5 Reactor Choice 16

1.6 Process Choice 17

References 19

Further Reading 19

2 Kinetics of Heterogeneous Catalytic Reactions 20
Rutger van Santen

2.1 Physical chemical principles 20

2.2 The Lock and Key Model, the Role of Adsorption Entropy 27

2.3 Equivalence of Electrocatalysis and Chemocatalysis 30

2.4 Microkinetics; the Rate-Determining Step 32

2.5 Elementary Rate Constant Expressions for Surface Reactions 34

2.6 The Pressure Gap 36

2.7 The Materials Gap 39

2.8 Coupling of Catalytic Reaction and Inorganic Solid Chemistry 42

2.9 In situ Generation of Organo-Catalyst 42

2.10 The Compensation Effect 44

References 46

3 Kinetics in Homogeneous Catalysis 48
Detlef Heller

3.1 Principles of a Catalyst and Kinetic Description 48

3.2 Catalyst Activity 54

3.3 Catalyst Activation and Deactivation 58

References 64

4 Catalytic Reaction Engineering Principles 67
Albert Renken and Lioubov Kiwi-Minsker

4.1 Preface 67

4.2 Formal Kinetics of Catalytic Reactions 68

4.3 Mass and Heat Transfer Effects 77

4.4 Homogenous Catalysis in Biphasic Fluid/Fluid Systems 103

References 108

Part II The Chemistry of Catalytic Reactivity 111

5 Heterogeneous Catalysis 113
Rutger van Santen

5.1 General Introduction 113

5.2 Transition Metal Catalysis 114

5.3 Solid Acids and Bases 132

5.4 Reducible Oxides 143

References 150

6 Homogeneous Catalysis 152
Matthias Beller, Serafino Gladiali, and Detlef Heller

6.1 General Features 152

References 169

7 Biocatalysis 171
Uwe Bornscheuer

7.1 Introduction 171

7.2 Examples 176

7.3 Summary/Conclusions 194

References 194

8 Electrocatalysis 201
Timo Jacob

8.1 Introduction 201

8.2 Theory 203

8.3 Application to the Oxygen Reduction Reaction (ORR) on Pt(111) 207

8.4 Summary 212

References 213

9 Heterogeneous Photocatalysis 216
Guido Mul

9.1 Introduction 216

9.2 Applications of Photocatalysis 219

9.3 Case Studies 220

9.4 Concluding Remarks 228

References 228

Part III Industrial Catalytic Conversions 231
10 Carbonylation Reactions 233

Matthias Beller

10.1 General Aspects 233

10.2 Hydroformylation 234

10.3 Other Carbonylations of Olefins and Alkynes 238

10.4 Carbonylations of Alcohols and Aryl Halides 244

References 246

11 Biocatalytic Processes 250
Uwe Bornscheuer

11.1 Introduction 250

11.2 Examples 253

11.2.1 General Applications 253

11.3 Case Study: Synthesis of Lipitor Building Blocks 257

11.4 Conclusions 259

References 259

12 Polymerization 261
Vincenzo Busico

12.1 Introduction 261

12.2 Polyolefins in Brief 262

12.3 Olefin Polymerization Catalysts 264

12.4 Olefin Polymerization Process Technology 273

12.5 The Latest Breakthroughs 280

References 285

13 Ammonia Synthesis 289
Jens Rostrup-Nielsen

13.1 Ammonia Plant 289

13.2 Synthesis 291

13.3 Steam Reforming 295

13.4 Conclusions 299

Abbreviations 299

References 299

14 Fischer–Tropsch Synthesis in a Modern Perspective 301
Hans Schulz

14.1 Introduction 301

14.2 Stoichiometry and Thermodynamic Aspects 304

14.3 Processes and Product Composition 308

14.4 Catalysts, General 311

14.5 Reaction Fundamentals 313

14.6 Concluding Remarks 323

References 323

15 Zeolite Catalysis 325
Rutger van Santen

15.1 Introduction 325

15.2 The Hydrocracking Reaction; Acid Catalysis 325

15.3 Lewis Acid–Lewis Base Catalysis; Hydrocarbon Activation 332

15.4 Selective Oxidation; Redox Catalysis 333

15.5 Framework-Substituted Redox Ions 335

References 339

16 Catalytic Selective Oxidation –Fundamentals, Consolidated Technologies, and Directions for Innovation 341
Fabrizio Cavani

16.1 Catalytic Selective Oxidation: Main Features 341

16.2 Catalytic Selective Oxidation: What Makes the Development of an Industrial Process More Challenging (and Troublesome) than Other Reactions 353

16.3 Catalytic Selective Oxidation: the Forefront in the Continuous Development of More-Sustainable Industrial Technologies 355

16.4 The Main Issue in Catalytic Oxidation: the Control of Selectivity 356

16.5 Dream Reactions in Catalytic Selective Oxidation: a Few Examples (Some Sustainable, Some Not Sustainable) 359

16.6 A New Golden Age for Catalytic Selective Oxidation? 361

16.7 Conclusions: Several Opportunities for More Sustainable Oxidation

Processes 363

References 363

17 High-Temperature Catalysis: Role of Heterogeneous, Homogeneous, and Radical Chemistry 365
Olaf Deutschmann

17.1 Introduction 365

17.2 Fundamentals 366

17.3 Applications 372

17.4 Hydrogen Production from Logistic Fuels by High-Temperature Catalysis 378

17.5 High-Temperature Catalysis in Solid Oxide Fuel Cells 380

References 385

18 Hydrodesulfurization 390
Roel Prins

18.1 Introduction 390

18.2 Hydrodesulfurization 391

18.3 The C-X Bond-Breaking Mechanism 393

18.4 Structure of the Sulfidic Catalyst 393

18.5 Hydrodenitrogenation 397

18.6 Determination of Surface Sites 398

References 398

Part IV Catalyst Synthesis and Materials 399

19 Molecularly Defined Systems in Heterogeneous Catalysis 401
Fernando Rasc´on and Christophe Cop´eret

19.1 Introduction 401

19.2 Single Sites: On the Border between Homogeneous and Heterogeneous Catalysis 402

19.3 Conclusion and Perspectives 415

References 415

20 Preparation of Supported Catalysts 420
Krijn P. de Jong

20.1 Introduction 420

20.2 Support Surface Chemistry 422

20.3 Ion Adsorption 423

20.4 Impregnation and Drying 425

20.5 Deposition Precipitation 427

20.6 Thermal Treatment 428

References 429

21 Porous Materials as Catalysts and Catalyst Supports 431
Petra de Jongh

21.1 General Characteristics 431

21.2 Sol-gel and Fumed Silica 433

21.3 Alumina and Other Oxides 436

21.4 Carbon Materials 438

21.5 Zeolites 440

21.6 Ordered Mesoporous Materials 442

21.7 Metal-Organic Frameworks 442

21.8 Shaping 443

References 444

22 Development of Catalytic Materials 445
Manfred Baerns

22.1 Introduction 445

22.2 Fundamental Aspects 446

22.3 Micro-Kinetics and Solid-State Properties as a Knowledge Source in Catalyst Development 448

22.4 Combinatorial Approaches and High-Throughput Technologies in the Development of Solid Catalysts 453

References 459

Part V Characterization Methods 463

23 In-situ Techniques for Homogeneous Catalysis 465
Detlef Selent and Detlef Heller

23.1 Introduction 465

23.2 In-situ Techniques for Homogeneous Catalysis 466

23.3 Gas Consumption and Gas Formation 467

23.4 NMR Spectroscopy 470

23.5 IR-Spectroscopy 481

23.6 UV/Vis Spectroscopy 486

23.7 Summary 490

References 490

24 In-situ Characterization of Heterogeneous Catalysts 493
Bert Weckhuysen

24.1 Introduction 493

24.2 Some History, Recent Developments, and Applications 495

24.3 In situ Characterization of a Reactor Loaded with a Catalytic Solid 497

24.4 In situ Characterization at a Single Catalyst Particle Level 501

24.5 Concluding Remarks 511

Acknowledgments 511

References 511

25 Adsorption Methods for Characterization of Porous Materials 514
Evgeny Pidko and Emiel Hensen

25.1 Introduction 514

25.2 Physical Adsorption 514

25.3 Classification of Porous Materials 517

25.4 Adsorption Isotherms 517

25.5 The Application of Adsorption Methods 518

25.6 Theoretical Description of Adsorption 519

25.7 Characterization of Microporous Materials 524

25.8 Characterization of Mesoporous Materials 527

25.9 Mercury Porosimetry 533

25.10 Xenon Porosimetry 533

References 534

26 A Critical Review of Some ‘‘Classical’’ Guidelines for Catalyst Testing 536
Frits Dautzenberg

26.1 Introduction 536

26.2 Encouraging Effectiveness 536

26.3 Ensuring Efficiency 537

26.4 Concluding Remarks 552

Appendix A: Three-Phase Trickle-Bed Reactors 552

List of Symbols and Abbreviations 558

References 559

Part VI Catalytic Reactor Engineering 561
27 Catalytic Reactor Engineering 563

Albert Renken and Madhvanand N. Kashid

27.1 Introduction 563

27.2 Types of Catalytic Reactors 564

27.3 Ideal Reactor Modeling/Heat Management 575

27.4 Residence Time Distribution 587

27.5 Microreaction Engineering 602

References 625

Index 629

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Matthias Beller obtained his PhD at the University of Göttingen, Germany and completed a postdoctoral fellowship at the Massachusetts Institute of Technology in Cambridge, USA. Since 1998, he has been head of the Leibniz Institute for Organic Catalysis at University of Rostock. He is a member of the board of Dechema's Catalysis Section, the German Catalysis Competence Network ("ConNeCat") as well as the Innovationsagentur Mecklenburg-Vorpommern. He is also a member of the Association for Technical Sciences of the Union of German Academies of Sciences and Humanities.

Albert Renken obtained his academic degrees at the Technical University of Hanover, Germany. Professor Renken has been affiliated with ETH Lausanne, Switzerland since 1977. He is author of over 350 scientific publications in journals and books and of numerous patents. From 1992 to 2000, Albert Renken was science councillor of the Swiss National Science Foundation (SNF), and from 1996 to 2000 he served as chairman of the European Federation of Chemical Reaction Engineering Working Party.

Rutger Anthony van Santen gained his doctorate from the University of Leiden, Netherlands. He became Professor of Catalysis at the Eindhoven University of Technology, where he was also promoted to scientific director. In 1991 he became director of the Netherlands Institute of Research in Catalysis, and in 2005 he was made Royal Netherlands Academy of Science and Arts Professor. He is a member of the Royal Dutch Academy of Arts and Sciences, Dutch Academy of Engineering and is a Knight in the order of the Dutch Lion. Professor van Santen is the author or editor of 13 books, over 600 research papers and 22 patents, and has been awarded several national and international awards and visiting professorships.
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“Overall, this is a useful book for process chemists with the reservation that modern carbon-carbon bond forming catalytic reactions (Buchwald-Hartwig, Suzuki-Miyaura, Heck etc) are not covered.  The emphasis is definitely towards heterogenous catalysis.”  (Organic Process Research & Development Journal, 1 November 2012)

 

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